Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane
Abstract
Octahedral molecular sieve (OMS-2) refers to a one-dimensional 2 × 2 framework of octahedral manganese oxo units based on the cryptomelane-type framework. Herein, we describe a niobium (Nb) substituted mixed metal oxide of Nb and Mn where the cryptomelane-type framework is retained. These materials are hydrothermally synthesized from the reaction of potassium permanganate, manganese sulfate, and homogeneous niobium(V) precursors. Niobium incorporation up to 31 mol% can be achieved without destroying the one dimensional 2 × 2 framework. The yields of the materials vary between 70 and 90%. These materials are analyzed by powder XRD, BET isotherm, TEM, SEM, XRF, and XPS studies. The synthesized materials show promising activity in selective oxidation of methanol to dimethoxymethane (DMM) at 200 °C. Normalized activity correlations followed the trend 21% Nb-OMS-2 > 15% Nb-OMS-2 > 31% Nb-OMS-2 > 68% Nb-OMS-2 > K-OMS-2. A fluctuation in methanol conversion was observed around 125–150 °C in most samples, suggesting this to be a catalytically important temperature regime when forming active sites for DMM production.
- Authors:
-
- Department of Chemistry, University of Connecticut, Storrs, USA
- Corporate Strategic Research, ExxonMobil Research and Engineering Company, Annandale, USA
- Institute of Material Science, University of Connecticut, Storrs, USA
- Department of Chemistry, University of Connecticut, Storrs, USA, Institute of Material Science
- Publication Date:
- Research Org.:
- Univ. of Connecticut, Storrs, CT (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1574081
- Alternate Identifier(s):
- OSTI ID: 1598224
- Grant/Contract Number:
- FG02-86ER13622
- Resource Type:
- Published Article
- Journal Name:
- RSC Advances
- Additional Journal Information:
- Journal Name: RSC Advances Journal Volume: 9 Journal Issue: 56; Journal ID: ISSN 2046-2069
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Wasalathanthri, Niluka D., Guild, Curtis, Nizami, Quddus A., Dissanayake, Shanka L., He, Junkai, Kerns, Peter, Fee, Jared, Achola, Laura, Rathnayake, Dinithi, Weerakkody, Chandima, Suib, Steven L., and Nandi, Partha. Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane. United Kingdom: N. p., 2019.
Web. doi:10.1039/C9RA04804A.
Wasalathanthri, Niluka D., Guild, Curtis, Nizami, Quddus A., Dissanayake, Shanka L., He, Junkai, Kerns, Peter, Fee, Jared, Achola, Laura, Rathnayake, Dinithi, Weerakkody, Chandima, Suib, Steven L., & Nandi, Partha. Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane. United Kingdom. https://doi.org/10.1039/C9RA04804A
Wasalathanthri, Niluka D., Guild, Curtis, Nizami, Quddus A., Dissanayake, Shanka L., He, Junkai, Kerns, Peter, Fee, Jared, Achola, Laura, Rathnayake, Dinithi, Weerakkody, Chandima, Suib, Steven L., and Nandi, Partha. Mon .
"Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane". United Kingdom. https://doi.org/10.1039/C9RA04804A.
@article{osti_1574081,
title = {Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane},
author = {Wasalathanthri, Niluka D. and Guild, Curtis and Nizami, Quddus A. and Dissanayake, Shanka L. and He, Junkai and Kerns, Peter and Fee, Jared and Achola, Laura and Rathnayake, Dinithi and Weerakkody, Chandima and Suib, Steven L. and Nandi, Partha},
abstractNote = {Octahedral molecular sieve (OMS-2) refers to a one-dimensional 2 × 2 framework of octahedral manganese oxo units based on the cryptomelane-type framework. Herein, we describe a niobium (Nb) substituted mixed metal oxide of Nb and Mn where the cryptomelane-type framework is retained. These materials are hydrothermally synthesized from the reaction of potassium permanganate, manganese sulfate, and homogeneous niobium(V) precursors. Niobium incorporation up to 31 mol% can be achieved without destroying the one dimensional 2 × 2 framework. The yields of the materials vary between 70 and 90%. These materials are analyzed by powder XRD, BET isotherm, TEM, SEM, XRF, and XPS studies. The synthesized materials show promising activity in selective oxidation of methanol to dimethoxymethane (DMM) at 200 °C. Normalized activity correlations followed the trend 21% Nb-OMS-2 > 15% Nb-OMS-2 > 31% Nb-OMS-2 > 68% Nb-OMS-2 > K-OMS-2. A fluctuation in methanol conversion was observed around 125–150 °C in most samples, suggesting this to be a catalytically important temperature regime when forming active sites for DMM production.},
doi = {10.1039/C9RA04804A},
journal = {RSC Advances},
number = 56,
volume = 9,
place = {United Kingdom},
year = {Mon Oct 14 00:00:00 EDT 2019},
month = {Mon Oct 14 00:00:00 EDT 2019}
}
https://doi.org/10.1039/C9RA04804A
Web of Science
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